Among the variety of chiral building blocks for the preparation of optically active functional materials, amino acids and sugars stand out because of their versatile structures and functional groups. In these chiral units, intra- and intermolecular noncovalent interactions, such as hydrogen bonding and π-stacking, play significant roles in the generation of smart functions. This review summarizes the fabrication and functions of chiral conjugated polyacetylenes and polyarylene ethynylenes and chiral supramolecules based on these natural chiral compounds.